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High adsorption selectivity of activated carbon and carbon molecular sieve boosting CO_(2)/n_(2) and CH_(4)/n_(2) separation

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Chinese Journal of Chemical Engineering 2024年第3期67卷 282-297页

作者： Siang Chen Wenling wu Zhaoyang niu Deqi Kong Wenbin Li Zhongli Tang Donghui Zhang The Research Center of Chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Flue gas and coal bed methane are two important sources of greenhouse *** swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is *** this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and n_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 *** experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric *** the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>n_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is n_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-n_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular ***,the adsorption selectivity of CH_(4)/n_(2) and CO_(2)/n_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) *** study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.

关键词： Activated carbon Carbon molecular sieve Adsorbent evaluation Adsorption equilibrium and kinetics Heat of adsorption Selectivity

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Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-Con_(4)-rich carbon support

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Chinese Chemical Letters 2024年第5期35卷 265-271页

作者： Jin Long Xingqun Zheng Bin Wang Chenzhong wu Qingmei Wang Lishan Peng Guizhou University Key Laboratory of Green Chemical and Clean Energy Technology Guizhou University Engineering Research Center of Efficient Utilization for Industrial WasteInstitute of Dual-carbon and New Energy Technology Innovation and Development of Guizhou ProvinceSchool of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China College of Safety Engineering Chongqing University of Science&TechnologyChongqing 401331China Key Laboratory of Rare Earths Chinese Academy of SciencesGanjiang Innovation AcademyGanzhou 341119China

Developing platinum-group-metal(PGM)catalysts possessing strong metal-support interaction and controllable PGM size is urgent for the sluggish oxygen reduction reaction(ORR)in proton-exchange membrane fuel ***,we propose an in-situ self-assembled reduction strategy to successfully induce highly-dispersed sub-3nm platinum nanoparticles(Pt nPs)to attach on resin-derived atomic Co coordinated by n-doped carbon substrate(Pt/Co_(SA)-n-C)for *** be specific,the interfacial electron interaction effect,along with a highly robust Co_(SA)-n-C support endow the as-fabricated Pt/Co_(SA)-n-C catalyst with significantly enhanced catalytic properties,i.e.,a mass activity(MA)of 0.719 A/mgPt at 0.9 ViR-free and a reduction of 24.2%in MA after a 20,000-cycles *** functional theory(DFT)calculations demonstrate that the enhanced electron interaction between Pt and Co_(SA)-n-C support decreases the dband center of Pt,which is in favor of lowering the desorption energy of ^(*)OH on Pt/Co_(SA)-n-C surface and accelerating the formation of H_(2)O,thus enhance the instinct activity of ***,the higher binding energy between Pt and Co_(SA)-n-C compared to Pt and C indicates that the migration of Pt has been suppressed,which theoretically explains the improved durability of Pt/Co_(SA)-*** work offers an enlightenment on constructing composite Pt-based catalysts with multiple active sites.

关键词： Fuel cells Oxygen reduction reaction Platinum Single-Con_(4)-rich carbon support Metal-substrate interaction

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Oxidation Evolution and Activity Origin of n-Doped Carbon in the Oxygen Reduction Reaction

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Transactions of Tianjin University 2024年第4期30卷 369-379页

作者： Jiaqi wu Chuanqi Cheng Shanshan Lu Bin Zhang Yanmei Shi Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China School of Materials Science and Engineering Institute of New Energy MaterialsTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Science Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China

n-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively ***,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon ***,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not *** this study,we discover a two-step oxida-tion process of n-doped carbon during the *** fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of n and the formation of abundant oxygen-containing functional *** oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)***,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant *** also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.

关键词： Oxygen reduction reaction n-doped carbon Reaction path Structural evolution Oxidation in reduction

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Heteroatoms doped iron oxide-based catalyst prepared from zinc slag for efficient selective catalytic reduction of nO_(x) with nH_(3)

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International Journal of Coal Science & Technology 2024年第1期11卷 180-193页

作者： Jiale Liang Yaojun Zhang Hao Chen Licai Liu Panyang He Lei wu College of Materials Science and Engineering Xi’an University of Architecture and TechnologyXi’an710055China School of Chemistry and Chemical Engineering Xi’an University of Architecture and TechnologyXi’an710055China School of Resources Engineering Xi’an University of Architecture and TechnologyXi’an710055China

Excessive emissions of nitrogen oxides from flue gas have imposed various detrimental impacts on environment,and the development of denO_(x) catalysts with low-cost and high performance is an urgent *** oxide-based material has been explored for promising denO_(x) ***,the unsatisfactory low-temperature activity limits their practical *** this study,a series of excellent low-temperature denitrification catalysts(Ha-FeO_(x)/yZS)were prepared by acid treatment of zinc slag,and the mass ratios of Fe to impure ions was regulated by adjusting the acid ***-FeO_(x)/yZS showed high denitrification performance(>90%)in the range of 180–300℃,and the optimal nO conversion and n2 selectivity were higher than 95%at 250℃.Among them,the Ha-FeO_(x)/2ZS synthesized with 2 mol/L HnO3 exhibited the widest temperature window(175–350℃).The excellent denitrification performance of Ha-FeO_(x)/yZS was mainly attributed to the strong interaction between Fe and impurity ions to inhibit the growth of crystals,making Ha-FeO_(x)/yZS with amorphous structure,nice fine particles,large specific surface area,more surface acid sites and high chemisorbed *** in-situ DRIFT experiments confirmed that the SCR reaction on the Ha-FeO_(x)/yZS followed both Langmuir-Hinshelwood(L-H)mechanism and Eley-Rideal(E-R)*** present work proposed a high value-added method for the preparation of cost-effective catalysts from zinc slag,which showed a promising application prospect in nO_(x) removal by selective catalytic reduction with ammonia.

关键词： Flue gas nO_(x)removal Zinc slag-derived catalyst nH_(3)-SCR Catalysis activity

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Synergy of heterogeneous Co/ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ n-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo wu Ximing Yan Yuhe Liao Hu Li national Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by n-functionalization is fascinating for on-purpose valorization of ***,a Co/ni-based dual-atom catalyst ConiDA@nC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous *** synergistic catalysis of Co/ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical ***,the Coni_(DA)@nC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer *** in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value n-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion Heterogeneous catalysis Lignin Dual-atom catalyst Selective C-ocleavage

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Exosomal let-7a-5p derived from human umbilical cord mesenchymal stem cells alleviates coxsackievirus B3-induced cardiomyocyte ferroptosis via the SMAD2/ZFP36 signal axis

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Journal of Zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第5期25卷 422-437页

作者： Xin LI Yanan HU Yueting wu Zuocheng YAnG Yang LIU Hanmin LIU Department of Pediatric Pulmonology and Immunology West China Second University HospitalSichuan UniversityChengdu 610041China Key Laboratory of Birth Defects and Related Diseases of Women and Children(Sichuan University) Ministry of EducationChengdu 610041China nHC Key Laboratory of Chronobiology(Sichuan University) Chengdu 610041China The Joint Laboratory for Lung Development and Related Diseases of West China Second University Hospital Sichuan University and School of Life Sciences of Fudan UniversityWest China Institute of Women and Children's HealthWest China Second University HospitalSichuan UniversityChengdu 610041China Sichuan Birth Defects Clinical Research Center West China Second University HospitalSichuan UniversityChengdu 610041China Department of Pediatrics the Third Xiangya HospitalCentral South UniversityChangsha 410013China

Viral myocarditis(VMC)is one of the most common acquired heart diseases in children and ***,its pathogenesis is still unclear,and effective treatments are *** study aimed to investigate the regulatory pathway by which exosomes alleviate ferroptosis in cardiomyocytes(CMCs)induced by coxsackievirus B3(CVB3).CVB3 was utilized for inducing the VMC mouse model and cellular *** echocardiography,left ventricular ejection fraction(LVEF),and left ventricular fractional shortening(LVFS)were implemented to assess the cardiac *** CVB3-induced VMC mice,cardiac insufficiency was observed,as well as the altered levels of ferroptosis-related indicators(glutathione) peroxidase 4(GPX4),glutathione(GSH),and malondialdehyde(MDA).However,exosomes derived from human umbilical cord mesenchymal stem cells(hucMSCs-exo)could restore the changes caused by CVB3 ***-7a-5p was enriched in hucMSCs-exo,and the inhibitory ffect of hucMSCs-exoa-ie-pmimo on CVB3-induced ferroptosis was higher than that of hucMSCs-exommie n(nC:negative control).Mothers against decapentaplegic homolog 2(SMAD2)increased in the VMC group,while the expression of zinc-finger protein 36(ZFP36)***-7a-5p was confirmed to interact with SMAD2 messenger RnA(mRnA),and the SMAD2 protein interacted directly with the ZFP36 *** SMAD2 and overexpressing ZFP36 inhibited the expression of ferroptosis-related ***,the levels of GPX4,solute carrier family 7,member 11(SLC7A11),and GSH were lower in the SMAD2 overexpression plasmid(oe-SMAD2)+let-7a-5p mimic group than in the oe-nC+let-7a-5p mimic group,while those of MDA,reactive oxygen species(ROS),and Fe^(2+)*** conclusion,these data showed that ferroptosis could be regulated by mediating SMAD2 ***-let-7a-5p derived from hucMSCs could mediate SMAD2 to promote the expression of ZFP36,which further inhibited the ferroptosis of CMCs to alleviate CVB3-induced VMC.

关键词： Exosome Let-7a-5p Mothers against decapentaplegic homolog 2(SMAD2) Coxsackievirus B3(CVB3) Ferroptosis

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Design of Support Effect in the Catalytic Application of Ligand-Protect Gold Clusters

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Chinese Journal of Chemistry 2024年第1期42卷 73-86页

作者： Shuohao Li Shenguang Fu Yuqing Gong nuojie wu Lei Wang Liang Wang School of Safety Engineering China University of Mining and TechnologyXuzhouJiangsu 221116China Schoolof Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsu 225009 Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization China University of Mining and Technology XuzhouJiangsu 221008China

Ligand-protected gold(Au_(n))clusters sometimes need the removal of organic ligands to expose more active sites and reduce steric hindrance in catalytic reactions,and large amount of organic and inorganic materials usually need to be employed as supports to anchor Aun clusters through different interaction ***,less comprehensive summaries have been provided about the crucial contribution of various supports to the catalytic performance of the supported Aun ***,this review firstly summarizes synthesis methods(e.g.,impregnation and encapsulation processes)for the supported Aun cluster catalysts,and then mainly points out specific contributions of support effect in a great diversity of catalytic reactions,as well as deep interaction ***,opportunities and challenging issues will be stated towards supported Aun clusters,in terms of improving catalytic performance and structural stability of Aun clusters inthedemand of catalysis.

关键词： Gold clusters Synthesis Support effect Catalytic performance Interaction

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Allosteric DnAzyme-based encoder for molecular information transfer

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Chinese Chemical Letters 2024年第7期35卷 235-241页

作者： Minghao Hu Tianci Xie Yuqiang Hu Longjie Li Ting Wang Tongbo wu School of Pharmacy Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China Department of Oncology Tongji Hospital of Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China GI Cancer Research Institute Tongji HospitalHuazhong University of Science and TechnologyWuhan 430030China School of Life Science and Technology Wuhan Polytechnic UniversityWuhan 430023China State Key Laboratory of Bioelectronics National Demonstration Center for Experimental Biomedical Engineering EducationSchool of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China

Dynamic DnA nanotechnology plays a significant role in nanomedicine and information science due to its high programmability based on Watson-Crick base pairing and nanoscale *** DnA machines and networks have been widely used in various fields,including molecular imaging,biosensors,drug delivery,information processing,and logic *** serve as crucial components for information compilation and transfer,allowing the conversion of information from diverse application scenarios into a format recognized and applied by DnA ***,there are only a few encoder designs with DnA ***,the molecular priority encoder is hardly *** this study,we introduce allosteric DnAzyme-based encoders for information *** design of the allosteric domain and the recognition arm allows the input and output to be independent of each other and freely *** pre-packaged mode design achieves uniformity of baseline dynamics and dynamics *** also integrated non-nucleic acid molecules into the encoder through the aptamer design of the allosteric ***,we developed the 2^(n)-n encoder and the EndoⅣ-assisted priority encoder inspired by immunoglobulin's molecular structure and effector *** our knowledge,the proposed encoder is the first enzyme-free DnA encoder with DnA output,and the priority encoder is the first molecular priority encoder in the DnA reaction *** encoders avoid complex operations on a single molecule,and their simple structure facilitates their application in complex DnA circuits and biological scenarios.

关键词： DnAzyme Encoder nucleic acids DnA circuit DnA strand displacement Dynamic DnA nanotechnology

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Single-atom sites regulation by the second-shell doping for efficient electrochemical CO_(2)reduction

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Chinese Chemical Letters 2024年第9期35卷 360-363页

作者： Qian-Qian Tang Li-Fang Feng Zhi-Peng Li Shi-Hao wu Long-Shuai Zhang Qing Sun Mei-Feng wu Jian-Ping Zou Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China national-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China

nitrogen-doped carbon loaded single-atom catalysts(SACs)are promising candidates for electrocatalytic conversion of CO_(2)into high-valuable chemicals,and the modification of catalysts by heteroatom-doping strategy is an effective approach to enhance the CO_(2)reduction ***,the large difference exists in atomic radius between nitrogen atoms and the doped heteroatoms may lead to the poor stability of active *** this study,we have synthesized a ni single atom catalyst with S doping at the secondshell on the ultrathin carbon nanosheets support(ni-n_(4)-SC)by solid-phase *** S atom in the second-shell contributes to the higher efficiency of CO_(2)conversion at lower potentials while the ni-n_(4)-SC can be more *** experimental results and theoretical calculations indicate that the S atom in second-shell breaks the uniform charge distribution and reduces the free energy of hydrogenation,which can increase the adsorption of CO_(2),accelerate charge transfer,and reduce the reaction energy *** work reveals the close relationship between the second-shell and the electrocatalytic activity of single atom sites,which also provides a new perspective to design efficient single atom catalysts.

关键词： Single-atom catalyst Heteroatom-doping Second shell CO_(2)electroreduction Electronic structure regulation

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Enhanced SERS aptasensor for sensitive detection of saxitoxin based on HAuCl/HOreaction system and Pt/Au nanozyme

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Food Science and Human Wellness 2024年

作者： Yueqing Li Xuemei Tang Wei Zeng Ting wu Long wu School of Food Science and Engineering， Key Laboratory of Tropical Fruits and Vegetables Quality and Safety for State Market Regulation， Hainan University

Saxitoxin （STX） is a marine biotoxin produced by cyanobacteria and methanobacteria， which is harmful to humans and aquatic organisms. Therefore， it is urgent to establish an efficient， sensitive and selective method for the screening of STX. In this paper， based on the HAuCl4/H2O2reaction system， gold nanoparticles （Au nPs） decorated Fe3O4magnetic beads (Fe3O4@Au nPs) and Pt/Au nanozymes （Pt/Au nZs）， an enhanced SERS aptasensor was proposed for sensitive and selective detection of STX. Firstly， SERS tag （4-MBA） and aptamer modified Fe3O4@Au nPs were hybridized with complementary DnA modified Pt/Au nZs （Pt/Au-cDnA） to form the specific complexes. Wherein， aptamer acted as capture agent to specifically recognize STX， Pt/Au nZs catalyzed HAuCl4/H2O2reaction to enhance SERS signal， and Fe3O4facilitated the magnetic separation and simple detection operations. The SERS aptasensor achieved sensitive detection of STX with a wide linear range from 0.02 μmol/L to 0.8 μmol/L and a low detection limit of 13 nmol/L （LOD， S/n=3）. To evaluate the performance of this method， STX were detected in the spiked seafood samples with recoveries from 78.75% to 150% with relative errors below 6.52%. Besides， the SERS aptasensor behaved good stability and repeatability， revealing its promising potential in STX detection and food safety detection.

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